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Coliform contamination of a coastal embayment: Sources and transport pathways

Fecal bacterial contamination of nearshore waters has direct economic impacts to coastal communities through the loss of shellfisheries and restrictions of recreational uses. We conducted seasonal measurements of fecal coliform (FC) sources and transport pathways contributing to FC contamination of Buttermilk Bay, a shallow embayment adjacent to Buzzards Bay, MA. Typical of most coastal embayments, there were no direct sewage discharges (i.e., outfalls), and fecal bacteria from human, domestic animal, and wildlife pools entered open waters primarily through direct deposition or after transport through surface waters or groundwaters. Direct fecal coliform inputs to bay waters occurred primarily in winter (December-March) from waterfowl, ~33 x 1012 FC yr-1 or ~67% of the total annual loading. Effects of waterfowl inputs on bay FC densities were mitigated by their seasonality, wide distribution across the bay surface, and the apparent limited dispersal from fecal pellets. On-site disposal of sewage by septic systems was the single largest FC source in the watershed-embayment system, 460 x 1012 FC yr-1, but due to attenuation during subsurface transport only a minute fraction, < 0.006 x 1012 FC yr-1, reached bay waters (<0.01% of annual input to bay). Instead, surface water flows, via storm drains and natural streams under both wet- and dry-weather conditions, contributed the major terrestrial input, 12 x 1012 FC yr-1 (24% of annual input), all from animal sources. Since most of the surface water FC inputs were associated with periodic, short-duration rain events with discharge concentrated in nearshore zones, wet-weather flows were found to have a disproportionately high impact on nearshore FC levels. Elution of FC from shoreline deposits of decaying vegetation (wrack) comprised an additional coliform source. Both laboratory and field experiments suggest significant elution of bacteria from wrack, ~3 x 1012 FC yr-1 on a bay-wide basis (6% of annual input), primarily by periodic tidal flooding and possibly by major rain events. Release of coliforms during resuspension of subtidal sediments was estimated to be a minor source in this system (<1.5 x 1012 FC yr-1 or < 3% of annual input), primarily associated with large storm events in the fall and winter. Based upon the relative source strengths and the spatial and temporal patterns of FC input to Buttermilk Bay, it appears that management practices in similar settings should account for migratory waterfowl, but remediation efforts should focus on the redirection of stormwater runoff through the groundwater transport pathway.

Environmental Science & Technology

Fungicides: An overlooked pesticide class?

Fungicides are indispensable to global food security and their use is forecasted to intensify. Fungicides can reach aquatic ecosystems and occur in surface water bodies in agricultural catchments throughout the whole growing season due to their frequent, prophylactic application. However, in comparison to herbicides and insecticides, the exposure to and effects of fungicides have received less attention. We provide an overview of the risk of fungicides to aquatic ecosystems covering fungicide exposure (i.e., environmental fate, exposure modelling, and mitigation measures) as well as direct and indirect effects of fungicides on microorganisms, macrophytes, invertebrates, and vertebrates. We show that fungicides occur widely in aquatic systems, that the accuracy of predicted environmental concentrations is debatable, and that fungicide exposure can be effectively mitigated. We additionally demonstrate that fungicides can be highly toxic to a broad range of organisms and can pose a risk to aquatic biota. Finally, we outline central research gaps that currently challenge our ability to predict fungicide exposure and effects, promising research avenues, and shortcomings of the current environmental risk assessment for fungicides.

Environmental Science & Technology

Antidepressant pharmaceuticals in two U.S. effluent-impacted streams: Occurrence and fate in water and sediment and selective uptake in fish neural tissue

Antidepressant pharmaceuticals are widely prescribed in the United States; release of municipal wastewater effluent is a primary route introducing them to aquatic environments, where little is known about their distribution and fate. Water, bed sediment, and brain tissue from native white suckers (Catostomus commersoni)were collected upstream and atpoints progressively downstream from outfalls discharging to two effluentimpacted streams, Boulder Creek (Colorado) and Fourmile Creek (Iowa). A liquid chromatography/tandem mass spectrometry method was used to quantify antidepressants, including fluoxetine, norfluoxetine (degradate), sertraline, norsertraline (degradate), paroxetine, Citalopram, fluvoxamine, duloxetine, venlafaxine, and bupropion in all three sample matrices. Antidepressants were not present above the limit of quantitation in water samples upstream from the effluent outfalls but were present at points downstream at ng/L concentrations, even at the farthest downstream sampling site 8.4 km downstream from the outfall. The antidepressants with the highest measured concentrations in both streams were venlafaxine, bupropion, and Citalopram and typically were observed at concentrations of at least an order of magnitude greater than the more commonly investigated antidepressants fluoxetine and sertraline. Concentrations of antidepressants in bed sediment were measured at ng/g levels; venlafaxine and fluoxetine were the predominant chemicals observed. Fluoxetine, sertraline, and their degradates were the principal antidepressants observed in fish brain tissue, typically at low ng/g concentrations. Aqualitatively different antidepressant profile was observed in brain tissue compared to streamwater samples. This study documents that wastewater effluent can be a point source of antidepressants to stream ecosystems and that the qualitative composition of antidepressants in brain tissue from exposed fish differs substantially from the compositions observed in streamwater and sediment, suggesting selective uptake.

Colorado, Iowa

Regional effects of agricultural conservation practices on nutrient transport in the Upper Mississippi River Basin

Despite progress in the implementation of conservation practices, related improvements in water quality have been challenging to measure in larger river systems. In this paper we quantify these downstream effects by applying the empirical U.S. Geological Survey water-quality model SPARROW to investigate whether spatial differences in conservation intensity were statistically correlated with variations in nutrient loads. In contrast to other forms of water quality data analysis, the application of SPARROW controls for confounding factors such as hydrologic variability, multiple sources and environmental processes. A measure of conservation intensity was derived from the USDA-CEAP regional assessment of the Upper Mississippi River and used as an explanatory variable in a model of the Upper Midwest. The spatial pattern of conservation intensity was negatively correlated ( p = 0.003) with the total nitrogen loads in streams in the basin. Total phosphorus loads were weakly negatively correlated with conservation ( p = 0.25). Regional nitrogen reductions were estimated to range from 5 to 34% and phosphorus reductions from 1 to 10% in major river basins of the Upper Mississippi region. The statistical associations between conservation and nutrient loads are consistent with hydrological and biogeochemical processes such as denitrification. The results provide empirical evidence at the regional scale that conservation practices have had a larger statistically detectable effect on nitrogen than on phosphorus loadings in streams and rivers of the Upper Mississippi Basin.

Environmental Science & Technology

Contaminant trends in reservoir sediment cores as records of influent stream quality

When reconstructing water-quality histories from lake and reservoir cores, it is sometimes assumed that the chemical signatures in the cores reflect historical water quality in the influent streams. To investigate this assumption, concentrations of metals, PAHs, and organochlorine compounds in sediment cores were compared to those associated with an influent-stream suspended sediment for three reservoirs in Fort Worth, TX, and two reservoirs in Boston, MA, U.S.A., and interpreted in light of land-use and regulation histories. In evaluating relations between suspended sediments and cores, three levels of preservation were indicated: (1) influent concentrations and historical trends are preserved in cores (metals at all sites; some organic contaminants at some sites); (2) some loss occurs during transport and initial deposition but relative historical trends are preserved in cores (some organic contaminants at some sites); and (3) neither stream concentrations nor relative historical trends are preserved (dieldrin and p,p???-DDT). The degree of preservation of influent concentration histories varied between lakes, particularly for PAHs. The results support the use of sediment cores to infer streamwater-quality histories for many contaminants but indicate that reservoir-bottom sediment samples might underestimate concentrations of organic contaminants in some streams.

Environmental Science & Technology

Archive of digital boomer seismic reflection data collected during USGS field activity 02LCA02 in Lakes Ada, Crystal, Jennie, Mary, Rice, and Sylvan, Central Florida, July 2002

In July of 2002, the U.S. Geological Survey and St. Johns River Water Management District (SJRWMD) conducted geophysical surveys in Lakes Ada, Crystal, Jennie, Mary, Rice, and Sylvan, central Florida, as part of the USGS Lakes and Coastal Aquifers (LCA) study. This report serves as an archive of unprocessed digital boomer seismic reflection data, trackline maps, navigation files, Geographic Information System (GIS) files, and formal Federal Geographic Data Committee (FGDC) metadata. Filtered and gained (a relative increase in signal amplitude) digital images of the seismic profiles are also provided. Refer to the Acronyms page for expansions of acronyms and abbreviations used in this report. The archived trace data are in standard Society of Exploration Geophysicists (SEG) SEG-Y format (Barry and others, 1975) and may be downloaded and processed with commercial or public domain software such as Seismic Unix (SU). Example SU processing scripts and USGS software for viewing the SEG-Y files (Zihlman, 1992) are also provided. The USGS Florida Integrated Science Center (FISC) - St. Petersburg assigns a unique identifier to each cruise or field activity. For example, 02LCA02 tells us the data were collected in 2002 for the Lakes and Coastal Aquifers (LCA) study and the data were collected during the second field activity for that study in that calendar year. Refer to http://walrus.wr.usgs.gov/infobank/programs/html/definition/activity.html for a detailed description of the method used to assign the field activity ID. The boomer plate is an acoustic energy source that consists of capacitors charged to a high voltage and discharged through a transducer in the water. The transducer is towed on a sled floating on the water surface and when discharged emits a short acoustic pulse, or shot, which propagates through the water, sediment column, or rock beneath. The acoustic energy is reflected at density boundaries (such as the seafloor, sediment, or rock layers beneath the seafloor), detected by the receiver, and recorded by a PC-based seismic acquisition system. This process is repeated at timed intervals (for example, 0.5 s) and recorded for specific intervals of time (for example, 100 ms). In this way, a two-dimensional (2-D) vertical profile of the shallow geologic structure beneath the ship track is produced. Figure 1 displays the acquisition geometry. Refer to table 1 for a summary of acquisition parameters. Table 2 lists trackline statistics. The unprocessed seismic data are stored in SEG-Y format (Barry and others, 1975). For a detailed description of the data format, refer to the SEG-Y Format page. See the How To Download SEG-Y Data page for download instructions. The printable profiles provided here are GIF images that were filtered and gained using Seismic Unix software. Refer to the Software page for details about the processing and examples of the processing scripts. The processed SEG-Y data were exported to Chesapeake Technology, Inc. (CTI) SonarWeb software to produce an interactive Web page of the profile, which allows the user to obtain a geographic location and depth from the profile for a curser position. This information is displayed in the status bar of the browser.

Florida

Development of the permeability/performance reference compound approach for in situ calibration of semipermeable membrane devices

Permeability/performance reference compounds (PRCs) are analytically noninterfering organic compounds with moderate to high fugacity from semipermeable membrane devices (SPMDs) that are added to the lipid prior to membrane enclosure. Assuming that isotropic exchange kinetics (IEK) apply and that SPMD-water partition coefficients are known, measurement of PRC dissipation rate constants during SPMD field exposures and laboratory calibration studies permits the calculation of an exposure adjustment factor (EAF). In theory, PRC-derived EAF ratios reflect changes in SPMD sampling rates (relative to laboratory data) due to differences in exposure temperature, membrane biofouling, and flow velocity-turbulence at the membrane surface. Thus, the PRC approach should allow for more accurate estimates of target solute/vapor concentrations in an exposure medium. Under some exposure conditions, the impact of environmental variables on SPMD sampling rates may approach an order of magnitude. The results of this study suggest that most of the effects of temperature, facial velocity-turbulence, and biofouling on the uptake rates of analytes with a wide range of hydrophobicities can be deduced from PRCs with a much narrower range of hydrophobicities. Finally, our findings indicate that the use of PRCs permits prediction of in situ SPMD sampling rates within 2-fold of directly measured values.

Environmental Science & Technology

Coastal strategies to predict Escherichia coli concentrations for beaches along a 35 km stretch of southern Lake Michigan

To understand the fate and movement of Escherichia coli in beach water, numerous modeling studies have been undertaken including mechanistic predictions of currents and plumes and empirical modeling based on hydrometeorological variables. Most approaches are limited in scope by nearshore currents or physical obstacles and data limitations; few examine the issue from a larger spatial scale. Given the similarities between variables typically included in these models, we attempted to take a broader view of E. coli fluctuations by simultaneously examining twelve beaches along 35 km of Indiana's Lake Michigan coastline that includes five point-source outfalls. The beaches had similar E. coli fluctuations, and a best-fit empirical model included two variables: wave height and an interactive term comprised of wind direction and creek turbidity. Individual beach R2 was 0.32-0.50. Data training-set results were comparable to validation results (R2 = 0.48). Amount of variation explained by the model was similar to previous reports for individual beaches. By extending the modeling approach to include more coastline distance, broader-scale spatial and temporal changes in bacteria concentrations and the influencing factors can be characterized. ?? 2008 American Chemical Society.

Environmental Science & Technology

In situ enhancement and isotopic labeling of biogenic coalbed methane

Subsurface microbial (biogenic) methane production is an important part of the global carbon cycle that has resulted in natural gas accumulations in many coal beds worldwide. Laboratory studies suggest that complex carbon-containing nutrients (e.g., yeast or algae extract) can stimulate methane production, yet the effectiveness of these nutrients within coal beds is unknown. Here, we use downhole monitoring methods in combination with deuterated water (D 2 O) and a 200-liter injection of 0.1% yeast extract (YE) to stimulate and isotopically label newly generated methane. A total dissolved gas pressure sensor enabled real-time gas measurements (641 days preinjection and for 478 days postinjection). Downhole samples, collected with subsurface environmental samplers, indicate that methane increased 132% above preinjection levels based on isotopic labeling from D 2 O, 108% based on pressure readings, and 183% based on methane measurements 266 days postinjection. Demonstrating that YE enhances biogenic coalbed methane production in situ using multiple novel measurement methods has immediate implications for other field-scale biogenic methane investigations, including in situ methods to detect and track microbial activities related to the methanogenic turnover of recalcitrant carbon in the subsurface.

Montana

Regenerable membrane sensors for ultrasensitive nanoplastic quantification enabled by a data-driven Raman spectral processing algorithm

The detection of nanoplastics (NPs) in complex natural water systems is hindered by matrix interferences and limitations in current analytical techniques. This study presents Pre_seg, a Raman spectral processing algorithm integrated with regenerable anodic aluminum oxide (AAO) membrane sensors, for ultrasensitive, rapid, and quantitative NP detection at the single-particle level. The AAO membranes function as both filtration substrates and Raman sensors, reducing sample loss and contamination. Pre_seg incorporates statistically determined thresholds for signal-to-noise ratios (SNRs) and full width at half maximums (fwhms) across segmented spectral ranges, effectively minimizing noise and enhancing accuracy and sensitivity of NP detection. Pre_seg achieved 93.5% prediction accuracy of NPs and ≥90.4% rejection accuracy for non-NP entries. Mixed NPs were quantified at the lowest concentration of 0.5 μg L –1 . The robustness of Pre_seg was validated in eutrophic and oligotrophic lake matrices following oxidation digestion pretreatment to mitigate organic interferences. Furthermore, the AAO membrane sensors demonstrated stability through multiple regeneration and reuse cycles. This innovative approach advances NP detection by enabling scalable, customizable, and environmentally relevant monitoring.

Environmental Science and Technology

Atmospheric processing of iron-bearing mineral dust aerosol and its effect on growth of a marine diatom, Cyclotella meneghiniana

Iron (Fe) is a growth-limiting micronutrient for phytoplankton in major areas of oceans and deposited wind-blown desert dust is a primary Fe source to these regions. Simulated atmospheric processing of four mineral dust proxies and two natural dust samples followed by subsequent growth studies of the marine planktic diatom Cyclotella meneghiniana in artificial sea-water (ASW) demonstrated higher growth response to ilmenite (FeTiO 3 ) and hematite (α-Fe 2 O 3 ) mixed with TiO 2 than hematite alone. The processed dust treatment enhanced diatom growth owing to dissolved Fe (DFe) content. The fresh dust-treated cultures demonstrated growth enhancements without adding such dissolved Fe. These significant growth enhancements and dissolved Fe measurements indicated that diatoms acquire Fe from solid particles. When diatoms were physically separated from mineral dust particles, the growth responses become smaller. The post-mineralogy analysis of mineral dust proxies added to ASW showed a diatom-induced increased formation of goethite, where the amount of goethite formed correlated with observed enhanced growth. The current work suggests that ocean primary productivity may not only depend on dissolved Fe but also on suspended solid Fe particles and their mineralogy. Further, the diatom C. meneghiniana benefits more from mineral dust particles in direct contact with cells than from physically impeded particles, suggesting the possibility for alternate Fe-acquisition mechanism/s.

Environmental Science & Technology

Trends in hydrophobic organic contaminants in urban and reference lake sediments across the United States, 1970-2001

A shift in national policy toward stronger environmental protection began in the United States in about 1970. Conversely, urban land use, population, energy consumption, and vehicle use have increased greatly since then. To assess the effects of these changes on water quality, the U.S. Geological Survey used sediment cores to reconstruct water-quality histories for38 urban and reference lakes across the United States. Cores were age-dated, and concentration profiles of polycyclic aromatic hydrocarbons (PAHs) and chlorinated hydrocarbons were tested statistically. Significant trends in total DDT, p,p???-DDE, and total PCBs were all downward. Trends in chlordane were split evenly between upward and downward, and trends in PAHs were mostly upward. Significant trends did not occur in about one-half of cases tested. Concentrations of p,p???-DDE, p,p???-DDD, and PCBs were about one-half as likely to exceed the probable effect concentration (PEC), a sediment quality guideline, in sediments deposited in the 1990s as in 1965-1975, whereas PAHs were twice as likely to exceed the PEC in the more recently deposited sediments. Concentrations of all contaminants evaluated correlated strongly with urban land use. Upward trends in PAH concentrations, the strong association of PAH with urban settings, and rapid urbanization occurring in the United States suggest that PAHs could surpass chlorinated hydrocarbons in the threat they pose to aquatic biota in urban streams and lakes.

Environmental Science & Technology

Accumulation of contaminants in fish from wastewater treatment wetlands

Increasing demands on water resources in arid environments make reclamation and reuse of municipal wastewater an important component of the water budget. Treatment wetlands can be an integral part of the water-reuse cycle providing both water-quality enhancement and habitat functions. When used for habitat, the bioaccumulation potential of contaminants in the wastewater is a critical consideration. Water and fish samples collected from the Tres Rios Demonstration Constructed Wetlands near Phoenix, Arizona, which uses secondary-treated wastewater to maintain an aquatic ecosystem in a desert environment, were analyzed for hydrophobic organic compounds (HOC) and trace elements. Semipermeable membrane devices (SPMD) were deployed to investigate uptake of HOC. The wetlands effectively removed HOC, and concentrations of herbicides, pesticides, and organic wastewater contaminants decreased 40−99% between inlet and outlet. Analysis of Tilapia mossambica and Gambusia affinis indicated accumulation of HOC, including p,p ‘-DDE and trans -nonachlor. The SPMD accumulated the HOC detected in the fish tissue as well as additional compounds. Trace-element concentrations in whole-fish tissue were highly variable, but were similar between the two species. Concentrations of HOC and trace elements varied in different fish tissue compartments, and concentrations in Tilapia liver tissue were greater than those in the whole organism or filet tissue. Bioconcentration factors for the trace elements ranged from 5 to 58 000 and for the HOC ranged from 530 to 150 000.

Environmental Science & Technology

Geographic setting influences Great Lakes beach microbiological water quality

Understanding of factors that influence Escherichia coli (EC) and enterococci (ENT) concentrations, pathogen occurrence, and microbial sources at Great Lakes beaches comes largely from individual beach studies. Using 12 representative beaches, we tested enrichment cultures from 273 beach water and 22 tributary samples for EC, ENT, and genes indicating the bacterial pathogens Shiga-toxin producing E. coli (STEC), Shigella spp., Salmonella spp, Campylobacter jejuni/coli, and methicillin-resistant Staphylococcus aureus, and 108–145 samples for Bacteroides human, ruminant, and gull source-marker genes. EC/ENT temporal patterns, general Bacteroides concentration, and pathogen types and occurrence were regionally consistent (up to 40 km), but beach catchment variables (drains/creeks, impervious surface, urban land cover) influenced exceedances of EC/ENT standards and detections of Salmonella and STEC. Pathogen detections were more numerous when the EC/ENT Beach Action Value (but not when the Geometric Mean and Statistical Threshold Value) was exceeded. EC, ENT, and pathogens were not necessarily influenced by the same variables. Multiple Bacteroides sources, varying by date, occurred at every beach. Study of multiple beaches in different geographic settings provided new insights on the contrasting influences of regional and local variables, and a broader-scale perspective, on significance of EC/ENT exceedances, bacterial sources, and pathogen occurrence.

Great Lakes

Predictions of anthropogenic background PFAS concentrations in soil and relation to bedrock lithology and groundwater quality

Detectable concentrations of per- and polyfluoroalkyl substances (PFAS) have been observed in soils in remote areas and presumably originate from atmospheric deposition. These anthropogenic background concentrations may enable some PFAS to leach to groundwater at levels that exceed regulatory criteria for drinking water. However, anthropogenic background soil concentrations and their connection to groundwater are not well characterized. We developed a boosted regression tree model to predict perfluorooctanesulfonic acid (PFOS) and perfluorooctanoic acid (PFOA) concentrations in shallow soils across northern New England. Low soil pH was the most important predictor of elevated anthropogenic PFOS and PFOA concentrations in background soils, rather than potential PFAS sources, land use, or population density. Total organic carbon (TOC) was also an important predictor for PFOS soil concentrations. Model predictions indicate that 73% of the shallow soils within Maine, Vermont, and New Hampshire exceed New Hampshire’s Soil Remediation Standard for PFOS (0.5 ng/g) and 41% exceed the PFOA standard (0.4 ng/g). Analysis of soil model results and groundwater data suggests that areas with high soil pH are associated with higher groundwater detection frequencies, illustrating how areas with less retention in soil are, conversely, also areas with potentially greater groundwater vulnerability. Further analysis indicates that groundwater may be more vulnerable in calcareous lithologies.

Maine, New Hampshire, Vermont

Measurement and modeling of polychlorinated biphenyl bioaccumulation from sediment for the marine polychaete neanthes arenaceodentata and response to sorbent amendment

Bioaccumulation rates of polychlorinated biphenyls (PCBs) for the marine polychaete Neanthes arenaceodentata were characterized, including PCB uptake rates from water and sediment, and the effect of sorbent amendment to the sediment on PCB bioavailability, organism growth, and lipid content. Physiological parameters were incorporated into a biodynamic model to predict contaminant uptake. The results indicate rapid PCB uptake from contaminated sediment and significant organism growth dilution during time-series exposure studies. PCB uptake from the aqueous phase accounted for less than 3% of the total uptake for this deposit-feeder. Proportional increase of gut residence time and assimilation efficiency as a consequence of the organism's growth was assessed by PCB uptake and a reactor theory model of gut architecture. Pulse-chase feeding and multilabeled stable isotope tracing techniques proved high sediment ingestion rates (i.e., 6?10 times of dry body weight per day) indicating that such deposit-feeders are promising biological indicators for sediment risk assessment. Activated carbon amendment reduced PCB uptake by 95% in laboratory experiments with no observed adverse growth effects on the marine polychaete. Biodynamic modeling explained the observed PCB body burdens for N. arenaceodentata, with and without sorbent amendment.

Environmental Science & Technology

Butyltin residues in southern sea otters (Enhydra lutris nereis) found dead along California coastal waters

Tributyltin (TBT) and its degradation products, mono- (MBT) and dibutyltin (DBT), were determined in liver, kidney, and brain tissues of adult southern sea otters (Enhydra lutris nereis) found dead along the coast of California during 1992a??1996. Hepatic concentrations of butyltin compounds (BTs = MBT + DBT + TBT) ranged from 40 to 9200 ng/g wet wt, which varied depending on the sampling location and gender. Concentrations of BTs in sea otters were comparable to those reported in stranded bottlenose dolphins from the U.S. Atlantic Coast during 1989a??1994. Greater accumulation of butyltins in sea otters was explained by their bottom-feeding habit and the diet that consists exclusively of invertebrates such as mollusks and gastropods. Livers of female sea otters contained approximately 2-fold greater concentrations of BTs than did those of males. The composition of butyltin compounds in sea otter tissues was predominated by TBT in most cases and suggestive of recent exposure. Large harbors such as Monterey Harbor that handle ships legally painted with TBT-containing antifouling paints continued to experience ecotoxicologically significant butyltin contamination. Sea otters, which were affected by infectious diseases, contained greater concentrations of BTs in their tissues than those that died from trauma and other unknown causes.

Californnia

Declining acidic deposition begins reversal of forest-soil acidification in the northeastern U.S. and eastern Canada

Decreasing trends in acidic deposition levels over the past several decades have led to partial chemical recovery of surface waters. However, depletion of soil Ca from acidic deposition has slowed surface water recovery and led to the impairment of both aquatic and terrestrial ecosystems. Nevertheless, documentation of acidic deposition effects on soils has been limited, and little is known regarding soil responses to ongoing acidic deposition decreases. In this study, resampling of soils in eastern Canada and the northeastern U.S. was done at 27 sites exposed to reductions in wet SO 4 2 &ndash; deposition of 5.7&ndash;76%, over intervals of 8&ndash;24 y. Decreases of exchangeable Al in the O horizon and increases in pH in the O and B horizons were seen at most sites. Among all sites, reductions in SO 4 2 &ndash; deposition were positively correlated with ratios (final sampling/initial sampling) of base saturation ( P < 0.01) and negatively correlated with exchangeable Al ratios ( P < 0.05) in the O horizon. However, base saturation in the B horizon decreased at one-third of the sites, with no increases. These results are unique in showing that the effects of acidic deposition on North American soils have begun to reverse.

Environmental Science & Technology